Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries

Wangda Li, Andrei Dolocan, Pilgun Oh, Hugo Celio, Suhyeon Park, Jaephil Cho and Arumugam Manthiram ()
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Wangda Li: Materials Science and Engineering Program and Texas Materials Institute, the University of Texas at Austin
Andrei Dolocan: Materials Science and Engineering Program and Texas Materials Institute, the University of Texas at Austin
Pilgun Oh: Materials Science and Engineering Program and Texas Materials Institute, the University of Texas at Austin
Hugo Celio: Materials Science and Engineering Program and Texas Materials Institute, the University of Texas at Austin
Suhyeon Park: School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST)
Jaephil Cho: School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST)
Arumugam Manthiram: Materials Science and Engineering Program and Texas Materials Institute, the University of Texas at Austin

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: Abstract Undesired electrode–electrolyte interactions prevent the use of many high-energy-density cathode materials in practical lithium-ion batteries. Efforts to address their limited service life have predominantly focused on the active electrode materials and electrolytes. Here an advanced three-dimensional chemical and imaging analysis on a model material, the nickel-rich layered lithium transition-metal oxide, reveals the dynamic behaviour of cathode interphases driven by conductive carbon additives (carbon black) in a common nonaqueous electrolyte. Region-of-interest sensitive secondary-ion mass spectrometry shows that a cathode-electrolyte interphase, initially formed on carbon black with no electrochemical bias applied, readily passivates the cathode particles through mutual exchange of surface species. By tuning the interphase thickness, we demonstrate its robustness in suppressing the deterioration of the electrode/electrolyte interface during high-voltage cell operation. Our results provide insights on the formation and evolution of cathode interphases, facilitating development of in situ surface protection on high-energy-density cathode materials in lithium-based batteries.

Date: 2017
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DOI: 10.1038/ncomms14589

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